Non-Markovian and nonequilibrium phonon effects are believed to be key ingredients in the energy transfer in photosynthetic complexes, especially in complexes which exhibit a regime of intermediate exciton–phonon coupling. In this work, we utilize a recently developed measure for non-Markovianity to elucidate the exciton–phonon dynamics in terms of the information flow between electronic and vibrational degrees of freedom. We study the measure in the hierarchical equation of motion approach which captures strong coupling effects and nonequilibrium molecular reorganization. We propose an additional trace distance measure for the information flow that could be extended to other master equations. We find thatmore » for a model dimer system and for the Fenna–Matthews–Olson complex the non-Markovianity is significant under physiological conditions.« less

Energy transfer and exciton coupling in isolated B800-850 complexes from the purple sulfur bacterium Chromatium tepidum were studied by means of spectrally resolved absorbance difference spectroscopy with a time resolution of 200 fs. Energy transfer from bacteriochlorophyll (BChl) 800 to BChl 850 was found to occur with a time constant of 0.8-0.9 ps. Remarkably, the amplitude of the absorbance changes of BChl 850 was 4 times larger than that of BChl 800. By relating this result to the crystal structure of B800-850 complexes of Rhodopseudomonas acidophila, it was concluded that the spectral properties of BChl 850 are mainly determined bymore » strong exciton interactions between BChl 850 molecules in a circular symmetric arrangement, which lead to concentration of the oscillator strength in a few optically allowed transitions, corresponding to delocalized eigenstates. In BChl 850, a rapid red shift of the bleaching was observed. This relaxation process may be ascribed either to vibrational relaxation or exciton scattering. A similar red shift appears to occur in BChl 800. 26 refs., 5 figs.« less